Lithium-sulfur (Li–S) batteries, with their high theoretical specific capacity and energy density, are considered a promising alternative to current energy storage technologies. However, their practical application is hindered by the polysulfide shuttle effect, which leads to capacity fade and reduced coulombic efficiency. In this study we employs density functional theory (DFT) to explore the use of two-dimensional (2D) metallic transition metal dichalcogenides (TMDs), tantalum diselenide (TaSe2) and tantalum ditelluride (TaTe2), as anchoring materials for lithium polysulfides (LiPSs). Our findings reveal that these TMD monolayers exhibit a balanced binding affinity towards LiPSs, ranging from 1.20ev to 3.34eV (TaSe2) and from 2.35ev to 3.74eV (TaTe2). Notably, the decomposition barriers for Li2S on TaSe2 and TaTe2 are significantly lower than those of bulk Li2S with a value of 1.62eV and 1.54eV, suggesting these materials can facilitate rapid charge-discharge processes. The introduction of strain, simulating the expansion during lithiation, demonstrates that these monolayers maintain their adsorption capabilities, a crucial attribute for practical applications, with a increased decomposition barriers of 2.4eV(TaSe2) and 2.51eV(TaTe2). The catalytic activity of these monolayers for the sulfur reduction reaction (SRR) was evaluated, showing a spontaneous conversion mechanism for lithium-sulfur clusters, which is expected to enhance the overall performance of Li–S batteries. This study presents TaSe2 and TaTe2 as innovative and promising candidates for advanced Li–S battery applications, offering a perspective in addressing the critical challenges associated with the polysulfide shuttle effect.